Exfoliation and Optical Properties of S=1 Triangular Lattice Antiferromagnet NiGa$_2$S$_4$

TL;DR

This study successfully exfoliated the 2D S=1 triangular lattice antiferromagnet NiGa$_2$S$_4$, characterizing its optical and electronic properties across different thicknesses, revealing potential for magnetic vdW heterostructures.

Contribution

It demonstrates the exfoliation of NiGa$_2$S$_4$ into monolayers and provides detailed optical, electronic, and structural characterization as a function of thickness.

Findings

NiGa$_2$S$_4$ can be exfoliated into few-layer samples.

Monolayer NiGa$_2$S$_4$ remains a Mott insulator with a ~1.5 eV gap.

Optical and electronic properties vary with layer number.

Abstract

Two-dimensional (2D) van der Waals (vdW) materials have been an exciting area of research ever since scientists first isolated a single layer of graphene. Single layer magnetic materials can provide a pathway for vdW heterostructures with magnetic properties. While most of the magnetic vdW materials exhibit ordering transitions in the bulk, here we report a successful exfoliation of a triangular lattice S=1 antiferromagnet NiGa$_2$S$_4$, which already demonstrates exotic magnetism in the bulk material. We establish the number of layers of the material by atomic force microscopy (AFM) and detail a careful characterization using Raman and optical spectroscopy to demonstrate how the optical, electronic, and structural properties of NiGa$_2$S$_4$ change as a function of sample thickness. Optical measurements and electronic structure calculations of bulk versus monolayer NiGa$_2$S$_4$ confirm the material to be a Mott insulator with an electronic gap of about 1.5 eV, which slightly increases for layers below 10 L. We conclude with a theoretical analysis of the possibility of doping monolayer NiGa$_2$S$_4$ by proximity to a metal.